Cavity Manipulation of Attosecond Charge Migration in Conjugated Dendrimers

Abstract

Dendrimers are branched polymers with wide applications to photosensitization, photocatalysis, photodynamic therapy, photovoltaic conversion, and light sensor amplification. The primary step of numerous photophysical and photochemical processes in many molecules involves ultrafast coherent electronic dynamics and charge oscillations triggered by photoexcitation. This electronic wavepacket motion at short times where the nuclei are frozen is known as attosecond charge migration. We show how charge migration in a dendrimer can be manipulated by placing it in an optical cavity and monitored by time-resolved X-ray diffraction. Our simulations demonstrate that the dendrimer charge migration modes and the character of photoexcited wave function can be significantly influenced by the strong light-matter interaction in the cavity. This presents a new avenue for modulating initial ultrafast charge dynamics and subsequently controlling coherent energy transfer in dendritic nanostructures.